EP0281336B1 - Nichtvernetzte Schaumstoffzusammensetzung - Google Patents

Nichtvernetzte Schaumstoffzusammensetzung Download PDF

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Publication number
EP0281336B1
EP0281336B1 EP88301706A EP88301706A EP0281336B1 EP 0281336 B1 EP0281336 B1 EP 0281336B1 EP 88301706 A EP88301706 A EP 88301706A EP 88301706 A EP88301706 A EP 88301706A EP 0281336 B1 EP0281336 B1 EP 0281336B1
Authority
EP
European Patent Office
Prior art keywords
butene
weight
polymer
ethylene
foam
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired - Lifetime
Application number
EP88301706A
Other languages
English (en)
French (fr)
Other versions
EP0281336A3 (en
EP0281336A2 (de
Inventor
Haruhiko Tanaka
Fukashi Kagawa
Koji Nakashima
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Mitsui Petrochemical Industries Ltd
Shell USA Inc
Original Assignee
Mitsui Petrochemical Industries Ltd
Shell Oil Co
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Mitsui Petrochemical Industries Ltd, Shell Oil Co filed Critical Mitsui Petrochemical Industries Ltd
Priority to AT88301706T priority Critical patent/ATE96454T1/de
Publication of EP0281336A2 publication Critical patent/EP0281336A2/de
Publication of EP0281336A3 publication Critical patent/EP0281336A3/en
Application granted granted Critical
Publication of EP0281336B1 publication Critical patent/EP0281336B1/de
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J9/00—Working-up of macromolecular substances to porous or cellular articles or materials; After-treatment thereof
    • C08J9/0061—Working-up of macromolecular substances to porous or cellular articles or materials; After-treatment thereof characterized by the use of several polymeric components
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J2323/00—Characterised by the use of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Derivatives of such polymers
    • C08J2323/02—Characterised by the use of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Derivatives of such polymers not modified by chemical after treatment
    • C08J2323/18—Homopolymers or copolymers of hydrocarbons having four or more carbon atoms
    • C08J2323/20—Homopolymers or copolymers of hydrocarbons having four or more carbon atoms having four to nine carbon atoms
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J2423/00—Characterised by the use of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Derivatives of such polymers

Definitions

  • This invention relates to a composition suitable for producing a non-crosslinked foam composed of a major proportion of a 1-butene polymer, a minor proportion of an ethylene polymer and a blowing agent.
  • Plastics foam products find wide applications in the fields of automobiles, household appliances, packing members, clothes, food, medical products, as thermally insulating materials and cushioning materials by making use of their light weight, thermal insulating properties and cushioning properties.
  • foam products are generally light weight, thermal insulating properties and cushioning properties.
  • plastics materials used in foam products There are many plastics materials used in foam products.
  • typical thermoplastic resins are high-pressure low-density polyethylene and polystyrene. These resins have been used as foam products naturally by focussing attention on their mechanical properties but due largely to ease of expansion molding.
  • the high-pressure low-density polyethylene and polystyrene have excellent expandability, they have poor heat resistance, and their maximum use temperature is about 80°C to about 90°C; they cannot be used at a high temperature above 100°C.
  • polypropylene is excellent, but polypropylene alone can hardly give a uniform foam.
  • Japanese Patent Publication No. 40,167/1981 discloses a foam prepared from a mixture of 90 to 30% by weight of polypropylene and 10 to 70% by weight of polybutene-1.
  • the patent publication states that this foam has excellent heat resistance, high-temperature creep characteristics, mechanical strength and thermal insulating properties and is suitable for use as a thermally insulating material for high-temperature structures. It also states that when the mixing proportions of polypropylene and polybutene-1 fall outside the above-specified ranges, a good foam cannot be obtained.
  • Japanese Laid-Open Patent Application No. 129,025/1983 discloses a polyolefin foam prepared from a mixture of (a) 60 to 98% by weight of a propylene/ethylene block copolymer having a melt index of 0.5 to 2.0 and an ethylene content of 5 to 15%, (b) 1 to 20% by weight of polybutene or a butene copolymer having a melt index of 2 to 10, and (c) 1 to 20% by weight of low-density polyethylene having a melt index of 2 to 10.
  • EP-A-147 690 discloses foamed particles of a non-crosslinked resin mixture of 10 to 95% by weight of an alpha-olefin/propylene random copolymer and 90 to 5% by weight of an ethylene/propylene random copolymer.
  • the foams described in the above documents are, though excellent in heat resistance, poor in flexibility because they are too hard owing to mechanical properties of polypropylene, and cannot be used as thermally insulating materials of curved piping portions and packing materials of bottle closures requiring flexibility.
  • the foams are used as thermally insulating materials for clothes and cushioning materials of medical products, they are required to be better in flexibility and elastic recovery than the conventional foams.
  • poly-1-butene is a polyolefin resin having flexibility and heat resistance and excellent in high-temperature creep characteristics in particular.
  • a copolymer of 1-butene and another alpha-olefin is used in the field requiring flexibility and creep resistance because when the content of alpha-olefin increases, the melting point lowers and heat resistance also decreases but flexibility improves.
  • the 1-butene polymer thus possesses such excellent characteristics but is similar in viscoelasticity to polypropylene. Therefore, like polypropylene, the 1-butene polymer alone can hardly afford a uniform foam.
  • US-A-4,359,544 discloses a composition comprising a 1-butene polymer, as small as 0.02 to 5.0 % by weight of stearamide and as small as 0.02 to 5.0% by weight of high-density polyethylene, said composition having high crystallisability and providing a film having improved tensile strength, modulus of elasticity and creep resistance. Said U.S. Patent however makes no mention of foams.
  • An object of this invention is to provide a novel expandable composition that gives a non-crosslinked foam suitable for use as a thermally insulating material, a cushioning material and a capliner material having excellent flexibility, heat resistance, creep resistance, cushioning properties and hygienic properties.
  • an expandable composition for use in producing a non-crosslinked foam comprising
  • the invention also provides a non-crosslinked foam obtainable from the expandable composition.
  • the 1-butene polymer (A) used in this invention is a homopolymer of 1-butene or a copolymer composed of at least 70 mole%, preferably at least 80 mole%, of polymerized units of 1-butene and not more than 30 mole%, preferably not more than 20 mole%, of polymerized units of an olefin having 2 to 20 carbon atoms other than 1-butene.
  • Examples of another olefin having 2 to 20 carbon atoms include ethylene, propylene, 4-methyl-1-pentene, 1-hexene, 1-octene, 1-decene, 1-tetradecene and 1-octadecene.
  • the 1-butene polymer (A) is a crystalline polymer preferably having a melt flow rate [MFR(E):ASTM D1238, E] of 0.01 to 50 g/10 min., preferably 0.05 to 20 g/10 min.
  • MFR(E) melt flow rate
  • ASTM D1238, E melt flow rate
  • the ethylene polymer (B) is a homopolymer of ethylene or a copolymer composed of at least 90 mole%, preferably at least 95 mole% of polymerized units of ethylene and not more than 10 mole%, preferably not more than 5 mole% of polymerized units of an alpha-olefin having 3 to 20 carbon atoms.
  • alpha-olefin having 3 to 20 carbon atoms examples include propylene, 1-butene, 4-methyl-1-pentene, 1-hexene, 1-octene, 1-decene, 1-tetradecene and 1-octadecene.
  • the ethylene polymer (B) is preferably a polymer having a melt flow rate [MFR (E): ASTM D1238, E] of 0.01 to 50 g/10 min., preferably 0.03 to 30 g/10 min. Where MFR (E) is less than 0.01 g/10 min., melt extrusion is hard to perform at the time of expansion molding. Where it exceeds 50 g/10 min., melt viscosity is low and expandability is poor.
  • MFR (E) ASTM D1238, E
  • the ethylene polymer (B) is preferably a crystalline polymer and has a density of at least 0.920 g/cm3, preferably at least 0.940 g/cm3, more preferably at least 0.950 g/cm3.
  • blowing agent (C) used in this invention examples include evaporatable blowing agents, for example, fluorinated aliphatic hydrocarbons such as trichloromonofluoromethane and dichlorotetrafluoroethane, and aliphatic hydrocarbons such as propane, methyl chloride, isobutane, pentane and hexane; and decomposable blowing agents such as sodium bicarbonate, ammonium carbonate, azodicarbonamide, barium azodicarboxylate, N,N'-dinitrosopentamethylenetetramine, 4,4-oxybis(benzenesulfonyl hydrazide), diphenylsulfone-3,3-disulfonyl hydrazide, p-toluene-sulfonyl semicarbazide, trihydrazinotriazine and biurea.
  • fluorinated aliphatic hydrocarbons such as trichloromon
  • blowing agents can be used singly or in combination.
  • fluorinated aliphatic hydrocarbons such as dichlorotetrafluoroethane chemically stable and having a great evaporation latent heat
  • azodicarbonamide and sodium bicarbonate in which an amount of gas generated is large and a temperature of terminating formation of a gas is much lower than a heat deterioration starting temperature of a 1-butene polymer (A)/ethylene polymer (B) mixture.
  • the expandable composition of this preferably comprises 90 to 98% by weight of the 1-butene polymer (A) and 10 to 2% by weight of the ethylene polymer (B).
  • the composition may contain, in addition to the 1-butene polymer (A), the ethylene polymer (B) and the blowing agent (C), a low-crystallinity or amorphous olefin random copolymer in such amount as not to impair the objects of this invention, for example, not more than 20 parts by weight per 100 parts by weight of the mixture of the 1-butene polymer (A) and the ethylene copolymer (B).
  • Examples thereof are a propylene/1-butene random copolymer, a propylene/ethylene random copolymer, an ethylene/1-butene random copolymer, an elastomer such as an ethylene/propylene terpolymer, and other low-crystallinity polyolefins such as polypropylene, poly-4-methyl-pentene and an ethylene/vinyl acetate copolymer.
  • the amount of the blowing agent (C) is properly adjusted depending on an intended foam. It is 0.2 to 30 parts by weight, preferably 0.5 to 20 parts by weight based on the total weight, 100 parts by weight, of the 1-butene polymer (A) and the ethylene polymer (B). When the amount of the blowing agent (C) is less than 0.2 part by weight, it is unlikely that a foam having a good expansion ratio could be obtained.
  • a so-called extrusion foaming method can be taken wherein the composition comprising the 1-butene polymer (A), the ethylene polymer (B) and the blowing agent (C) is extruded from a die in molten or softened state to expand a gas generated from the blowing agent contained in the composition at high to normal pressures.
  • composition used in this invention can contain, besides the blowing agent, additives ordinarily used in polyolefins, such as heat-resistant stabilizers, slip agents and antistatic agents in such amounts as not to impair the objects of this invention.
  • additives ordinarily used in polyolefins such as heat-resistant stabilizers, slip agents and antistatic agents in such amounts as not to impair the objects of this invention.
  • the non-crosslinked foam obtained from the composition of this invention may be in various forms such as sheets, pipes, rods and tubes by properly changing a die of an extrusion molding machine.
  • the composition of this invention allows easy expansion molding without cross-linking compared to 1-butene polymer which is difficult to use in expansion molding without crosslinking.
  • the resulting foam of this invention is made of uniform, fine closed cells.
  • the composition is composed mainly of the 1-butene polymer, it is better than the ordinary high-pressure low-density polyethylene foam and polystyrene foam in heat resistance, flexibility, creep resistance, cushioning properties and hygienic properties.
  • These foams can properly be used in thermally insulating materials of high-temperature structures and packing materials requiring high-temperature sterilization treatment, such as bottle closures.
  • PB-I + HDPE a resin mixture
  • PB-1 a 1-butene homopolymer
  • HDPE high-density polyethylene
  • ADCA azodicarbonamide
  • the mixture was melt-kneaded in a single-screw extruder (screw diameter 40 mm, set temperature 190°C) and extruded from a pipe-forming die (set temperature 120°C) to form a pipe-like foam.
  • the resulting foam was of a smooth surface and had an apparent specific volume (volume/weight found from an external size) of 2.1 and a true specific volume (measured by an air compression picnometer of Beckman) of 2.0. It was a good foam made of uniform, fine closed cells.
  • Example 1 was repeated except that the proportion of HDPE was changed as shown in Table 1. As a result, a foam made of uniform, fine closed cells and having a smooth surface was obtained as shown in Table 1.
  • PB-II + HDPE a resin mixture
  • PB-II + HDPE a resin mixture
  • the mixture was then melt-kneaded in a single-screw extruder (screw diameter 40 mm; set temperature 190°C), and extruded from a pipe-forming die (set temperature 95°C) to afford a pipe-like foam.
  • the resulting foam was made of uniform, fine closed cells and had a smooth surface as shown in Table 1.
  • Example 1 was followed but using PB-I alone.
  • the cellular film of the obtained foam was broken, the surface was heavily uneven and the specific volume was low.
  • Example 1 was followed but using PB-I and HDPE in amounts shown in Table 1.
  • Example 4 was followed but using PB-II alone.
  • the cellular film of the obtained foam was broken, the surface was heavily uneven and the expansion ratio was low. Thus, the foam was not good.
  • Example 4 was followed but using PB-II and HDPE as shown in Table 1.
  • the surface of the obtained foam was not so heavily uneven as in Comparative Example 3 but had small raisings and depressions. Moreover, there was a big difference in apparent and true specific volumes of the foam, and the foam appeared to be open-cellular.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Manufacture Of Porous Articles, And Recovery And Treatment Of Waste Products (AREA)
  • Compositions Of Macromolecular Compounds (AREA)

Claims (3)

  1. Expandierbare Masse zur Verwendung zur Herstellung eines nicht-vernetzten Schaumstoffs, umfassend:
    (A) 80 bis 99 Gew.-% eines 1-Buten-Homopolymers oder eines 1-Buten-Copolymers, bestehend aus mindestens 70 mol% polymerisierten Einheiten von 1-Buten und nicht mehr als 30 mol% polymerisierte Einheiten eines Olefins mit 2 bis 20 Kohlenstoffatomen, außer 1-Buten, wobei das 1-Butenpolymer eine Schmelzflußrate von 0,01 bis 50 g/10 min aufweist,
    (B) 20 bis 1 Gew.-% eines Ethylen-Homopolymers oder eines Ethylen-Copolymers, bestehend aus mindestens 90 mol% polymerisierten Einheiten von Ethylen und nicht mehr als 10 mol% polymerisierten Einheiten eines α-Olefins mit 3 bis 20 Kohlenstoffatomen, wobei das Ethylenpolymer eine Schmelzflußrate von 0,01 bis 50 g/10 min aufweist, und
    (C) ein Treibmittel in einer Menge von 0,2 bis 30 Gew.-Teilen auf 100 Gew.-Teile Gesamtgewicht des 1-Butenpolymers (A) und des Ethylenpolymers (B), wobei die Prozentgehalte sich auf das Gesamtgewicht des 1-Butenpolymers (A) und des Ethylenpolymers (B) beziehen.
  2. Masse nach Anspruch 1, umfassend 90 bis 98 Gew.-% des 1-Butenpolymers (A) und 10 bis 2 Gew.-% des Ethylenpolymers (B).
  3. Nicht-vernetzter Schaumstoff, erhältlich aus einer Masse nach Anspruch 1 oder 2.
EP88301706A 1987-02-28 1988-02-26 Nichtvernetzte Schaumstoffzusammensetzung Expired - Lifetime EP0281336B1 (de)

Priority Applications (1)

Application Number Priority Date Filing Date Title
AT88301706T ATE96454T1 (de) 1987-02-28 1988-02-26 Nichtvernetzte schaumstoffzusammensetzung.

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP62044056A JPH07116309B2 (ja) 1987-02-28 1987-02-28 無架橋発泡体用組成物
JP44056/87 1987-02-28

Publications (3)

Publication Number Publication Date
EP0281336A2 EP0281336A2 (de) 1988-09-07
EP0281336A3 EP0281336A3 (en) 1990-03-07
EP0281336B1 true EP0281336B1 (de) 1993-10-27

Family

ID=12680956

Family Applications (1)

Application Number Title Priority Date Filing Date
EP88301706A Expired - Lifetime EP0281336B1 (de) 1987-02-28 1988-02-26 Nichtvernetzte Schaumstoffzusammensetzung

Country Status (5)

Country Link
US (2) US4791143A (de)
EP (1) EP0281336B1 (de)
JP (1) JPH07116309B2 (de)
AT (1) ATE96454T1 (de)
DE (1) DE3885122T2 (de)

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JPH0712648B2 (ja) * 1987-09-11 1995-02-15 三井石油化学工業株式会社 無架橋発泡体を基材とする積層体
JPH0755990B2 (ja) * 1989-11-02 1995-06-14 宇部興産株式会社 電線被覆用の発泡性ポリオレフィン樹脂組成物
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US5208266A (en) * 1992-04-28 1993-05-04 Toshimichi Yamazaki Lightly crosslinked polymeric foams and process for making same
DE4301601A1 (de) * 1993-01-22 1994-07-28 Chemie Linz Deutschland Flammfeste Kunststoffe mit einem Gehalt an Trihydrazinotriazin, Triguanidinotriazin oder deren Salzen
US5585411A (en) * 1993-08-11 1996-12-17 Shell Oil Company Plastic foams made from polybutylene blends
US5883144A (en) 1994-09-19 1999-03-16 Sentinel Products Corp. Silane-grafted materials for solid and foam applications
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JP3558422B2 (ja) * 1995-09-07 2004-08-25 三井化学株式会社 多層管
US5844009A (en) 1996-04-26 1998-12-01 Sentinel Products Corp. Cross-linked low-density polymer foam
CA2203595A1 (en) 1996-04-26 1997-10-26 Robert F. Hurley Cross-linked polyolefin tape
US5882776A (en) 1996-07-09 1999-03-16 Sentinel Products Corp. Laminated foam structures with enhanced properties
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CA2518756A1 (en) * 2003-01-21 2004-08-05 Robert Peterson Golf ball of unitary molded construction
JP4126491B2 (ja) * 2003-03-06 2008-07-30 住友化学株式会社 発泡性樹脂組成物およびプロピレン系樹脂発泡体
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US20090313865A1 (en) * 2008-06-20 2009-12-24 Stephen Vincent Peretti Scent delivery system for greeting cards, envelopes and bags
BE1020760A3 (fr) * 2012-06-21 2014-04-01 Nmc Sa Mousses a base de butene et d'ethylene.
CN107923217A (zh) 2015-02-13 2018-04-17 埃美斯博瑞集团有限公司 低压缩力的tpe耐候性密封件
PL3433317T3 (pl) 2016-03-24 2020-07-13 Basell Poliolefine Italia S.R.L. Miękka kompozycja poliolefinowa

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JPH0660255B2 (ja) * 1986-09-16 1994-08-10 三井石油化学工業株式会社 無架橋発泡体

Also Published As

Publication number Publication date
EP0281336A3 (en) 1990-03-07
US4791143A (en) 1988-12-13
ATE96454T1 (de) 1993-11-15
JPS63213531A (ja) 1988-09-06
DE3885122T2 (de) 1994-05-05
JPH07116309B2 (ja) 1995-12-13
US4918111A (en) 1990-04-17
DE3885122D1 (de) 1993-12-02
EP0281336A2 (de) 1988-09-07

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